DE2116359A1 - Catalyst bed and method of charging the catalyst - Google Patents

Description

Catalyst bed and method of charging the catalyst

The invention relates to a catalyst bed with increased bulk density and a method of charging a reactor with a solid catalyst and a method of charging Catalysts, by which the L'efficiency of the catalysts is improved.

In particular, the invention relates to a method of filling a solid catalyst in a fixed bed reactor, forming a catalyst surface with increased bulk density; In the process, solid catalyst particles, which have a practically cylindrical geometry on iron, with a perpendicular Filling speed of the reactor of up to 43 cm per i-.inu "GG una with an average fruien x> 'all abbr.nä der

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Catalyst particles through a gaseous medium to the catalyst surface of at least about 30.5 cm is charged into the reactor in a downward motion with the longitudinal axis aligns the catalyst strips in the catalyst bed essentially horizontally.

The invention also relates to a catalyst bed with increased bulk density per unit volume of a reactor, the solid catalyst texlchen a practically cylindrical geometry have, and wherein the cylindrical catalyst texlchen in the catalyst bed substantially horizontally, are directed.

Up to now, catalysts have usually been filled in using the so-called "sock" method. In this process, a funnel and a hose attached to it, which extends to the bottom of the reactor or to the surface of the catalyst, are used. The funnel and hose are charged with catalyst and the catalyst is discharged from the bottom of the hose by slowly lifting the hose. A cone is formed on the catalyst bed that is being formed, which can be distributed over a rake during the filling η, χΐ. The usual reactors, the dimensions of which vary from about 30.5 ^cm to 4-6 m in width and from about 1.5 to 21.3 mm in length, are loaded according to this "sock" technique. One of the problems that occurs when charging the reactors according to this process is that the catalyst bed can contain cavities, which can collapse during operation, local overheating caused by the exothermic reactions of the steeper oil deposits, and can lead to the need to use larger reactor volumes. Further, more time is box of · "sock" technique for loading ^a: le; KtüL's needs, as the tube through which the Katalysa * - is tor introduced into the reactor, continuously raised 'are muli, AEOI: iit the Catalyst can flow. Except after that

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The process described above can also be used continuously for the catalyst be filled in through a funnel, which also forms a cone, which, as in the above case, with the Rake can be distributed over the entire catalyst bed.

The collapse of the catalyst can change the total volume of the catalyst bed, thereby reducing devices such as e.g. Thermal wells that are inserted into the reactor for temperature measurement can be damaged. In addition, the collapse of the catalyst can damage the surface of the catalyst bed send up to a level where the Therrnoschacht is no longer in contact with the catalyst, which means that the reaction temperature is not monitored during a reaction can be. The problem of local "overheating, mainly due to poor distribution of the liquid flow evoked during exothermic reactions, this means that reactions occur under non-uniform temperature conditions take place, whereby undesirable side reactions take place and undesirable life products are generated.

Another problem that arises with the previous method for charging catalysts is that, for a given reactor volume, the amount of catalyst that can be charged is determined by the catalyst density ultimately achieved. The possibility of increasing the bulk density of the existing catalyst would therefore allow an increased rate of average ev i ..: setzunf-steeply at the same space velocity or the same throughput at lower space velocities. More intense reaction conditions and increased throughputs can be obtained for a given catalyst volume because the maximum bulk density of the catalyst can be achieved.

The aim of the Ürfindunr iat ciahor the increased Ausriutäimp; of catalysts in bed cactors.

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It has now been found that the catalyst utilization, liquid distribution and bulk density per unit volume of a reactor by a method of filling catalysts can be improved in a reactor in which solid catalyst particles have a practically cylindrical geometry have, with a vertical filling speed of the reactor of up to 4-3 cm per Iuinute and at an average free fall distance of the catalyst particles through a gaseous Kediura up to the catalyst surface of at least about 3G.5 cm in downward motion in The reactor can be charged with the catalyst particles being essentially horizontal in the catalyst surface relay a message.

In particular, it has been found that the inventive Process a substantial improvement in the bulk density that

the
approaches the maximum bulk density of the catalyst, can be achieved. In addition, the increased bulk density creates a solid catalyst bed with a much lower tendency to collapse, and the method according to the invention also achieves an orientation of the catalyst particles which approximates the completely horizontal orientation substantially, whereby a better distribution of the liquid flow and the horizontal mixing is achieved will. Also of importance is the fact that the process according to the invention permits the production of a catalyst bed with minimal formation of catalyst fines. The formation of catalyst abrasion is generally below 1%, based on the total volume of the catalyst introduced, and even below 0.5 vol .- ^ j.

In addition, by the method proposed above, the bulk density of the catalyst per unit volume of the reactor elevated. The use of the method according to the invention for filling catalysts has proven to be particularly advantageous

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for hydrogenation processes. The application of the invention Catalyst filling process enables an improved Hydrogenation process in which a hydrogenation catalyst according to the process according to the invention is introduced into a reactor and then hydrogen and the hydrogenatable organic material are brought into contact with the hydrogenation catalyst and a hydrogenated organic haterial is obtained. The hydrogenation process according to the invention thus enables a higher throughput for the same ratio of units by weight of starting material per unit weight of catalyst per Hour (weight hourly space velocity VJHSV) and a higher catalyst weight per reactor volume. The increase in density The catalyst also enables smaller and cheaper reactors to be built and used for a given throughput.

When carrying out the process according to the invention, the catalyst is introduced into the reactor in a downward direction. In general, reactors whose dimensions are from about 0.3 to about 4.6 m, preferably from about 0.9 to about 4 m in diameter and from about 1.5 to about 38 m, preferably from about 3 to about 21 m in length, can be according to the Inventive method fed v / ground. The catalyst is filled into the reactor at a vertical filling speed of up to about 43 cw per minute, preferably from about 2.54 cm to about 15.2 cm and especially from about 50 to 10.2 cm per minute . The. The reactor should, however, preferably be filled at a moderate speed, and after a level fill;: eHchv; i r.ui ir it; has been reached, an icne ! during the formation of the Ka bolyr,;. ¹ basket (job einfei ι alt en worcieii. Uio ■ catalystOL'teilcheri been in (lon .dcaKtcr na einoi iv.loho:! point; introduced that the distance to the t "fibnlyr. aboroberflücho, which forms during the Kataiyj - ;;. ibofl; - i Louen dui-cli a p; as-

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Shaped medium are introduced, allowed on average a free fall of the catalyst particles for at least about 30.5 cm, preferably about 1.5 to about 3 &, 1 m and especially from about 3 to about 21 m .. The gaseous hedium is generally air or , depending on the specific catalyst used, also an inert medium ν; ie for example nitrogen. The minimum free fall distance generally ensures a sufficient downward speed to align the Kätalysatorteilchen along their major axis, that is, the free fall distance should be large enough so that the catalyst particle can move a little vertically upwards after touching the catalyst surface, whereby the correct one Alignment is done. Therefore, the catalyst particles normally fall one by one onto the catalyst surface while the catalyst bed is being formed. In this ^T 7eise virtually completely horizontal orientation of the catalyst is achieved. The term "virtually perfectly horizontal orientation" means that the most likely orientation of the longitudinal axis of the catalyst particles is the horizontal orientation. Furthermore, the practically completely horizontally oriented catalyst particles, according to the definition used here, result in a catalyst surface in which the difference between the highest and the deepest point is less than 10 / i of the diameter of the ivatcilysis bed, i.e. it becomes a practical one A flat surface whose height difference is preferably less than 5 % , especially less than 1%.

Uio ubi _; ; en.-ai.zbexi with regard to the i'Villgesciiwiriai £ K.eit, the free i ^ ll & bstanaes and the horizontal orientation; the catalyst particles within the ranges given above are preferred, d; · :: ie - .. ine _t rakt-ipch completely horizontal

l: · der j ·.? .. L Ox ^ f ₁ at ο steep hen ensure, while: i "bi ;; uiu the maximum achievable iiehütbuiente for a given catalyst bed is practically achieved.

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th factor dimensions correspond to those usually used for technical Processes such as hydrogenation, catalytic cracking and Iiydrocracivungen used reactor dimensions.

In general, the process according to the invention can be applied to catalyst particles which have a practically cylindrical geometry, it being particularly suitable for extruded catalyst particles. lr.1 In general, the diameter of the particles should not be less than 3 ^ of the diameter of the reactor; the particles normally have a diameter of about,? ¹ ", '^ Bim to etv; a 6.55 ^imn » preferably about 1.5 ^ 7 nim to about ;;, 1? ^ I- »m, with the lungs in the ranges given above compared to the diameter of the owls something Ί, 5 to about o times, preferably about 2 to 5 times.

The catalyst can be fed into the reactor in various ways as long as the above procedural requirements are adhered to be, r-for example, the milia can be served by a multiple perforated disc, the same area as the one to be formed Has catalyst bed, and with the aid of which the catalyst be distributed over the entire i \ atalysato ^ surface Can be introduced.

Line before ^ u.-tc working method for filling the catalyst in the reactor consists äarin, dal; can be a common funnel used, soft an inverted cone with an opening the öpit ^ e is the cone. Un an even distribution of the Reaching particles becomes a hollow, conical manifold (e.g. i). a cone) attached to the Trich-cer outlet opening. the vertical height of the conical distributor can be regulated by an adjusting device, e.g. by a threaded rod, which passed through aio putty of the distributor and the funnel will. The tip of the conical manifold is centered in the outlet opening of the funnel. The vertical position of the conical distributor is adjusted to allow the catalyst to flow and thus regulates the flow of the catalyst

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zero to different E ¹ UlIp: speed of the reactor. The conical manifold is a cone which has a plurality of evenly spaced orifices on the surface of the cone at a point below the funnel outlet opening to the base, their length from about 2.54 cm to about 50.0 cm and their width varies from about 6.35 mm to about 2.54 cm. The surface of the conical manifold typically has from about 4 to about 24 openings. The size of the conical manifold depends on the size of the reactor to be charged, and generally has a tip to base length of about 15 »24- cm to about 4-5.7 cm and a diameter at the base of about 15» 24- cm to about 45.7 cm The dimensions of the conical manifold and openings are adjusted to accommodate the catalyst can flow from the funnel along the surface of the conical distributor to the base of the conical distributor and through the openings at such a rate that the uniform distribution of the catalyst particles over the surface area of the reactor and the catalyst surface to be formed is ensured.

A variety of solid catalysts can, according to the invention Processes are filled, e.g. oxidation, Ilydro-desulphurization, kydrocracking, grazing, recovery and Hydrogenation catalysts. Typical examples of desulfurization catalysts are the transition rivets, metal oxides, iietailulfide or other metal salts, prefer the hydrodesulfurization catalyze, and that by hydrogen sulfide or other sulfur compounds are not poisoned. the preferred catalysts are the oxides and / or sulfides, e.g. the oxides or sulfides of molybdenum, tungsten, quiet, cobalt, Windings, chrome and the like. Vanadium compounds can can also be used in some cases. Line special active combination consists of an oxide or a sulfide one Metal from group VIB with an oxide or sulfide one ! Group VIII metal. Combinations, e.g.

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Molybdenum and cobalt oxide, or holybdenum oxide and iMXckeloxid, Tungsten sulfide and wound sulfide, and the like can be used.

A particularly active catalyst consists of the cobalt molybdate known substance, which should actually be a mixture of cobalt oxide and wolybdenum oxide, with the atomic ratio of Co to Ho can be between about 0.4 and 5 »0. This catalyst or one of the other above catalysts can be in unsupported B'orm or otherwise on a suitable adsorbent Oxide carriers such as aluminum oxide, silicon dioxide, zirconium dioxide, i'horium dioxide, magnesium oxide, titanium dioxide, Bauxite, acid activated clays, or a combination thereof can be used.

are typical examples of hydrocracking catalysts crystalline aluminum silicate zeolites, which are an i.etall from the platinum group (e.g. platinum or palladium) in the form deposited or compounded thereon. Liese Crystalline zeolites are characterized by their very ordered crystal structure and uniform pores, whereby they have an anionic aluminum silicate cage structure, in which aluminum oxide and silicon dioxide tetrahedra are arranged in intimate connection with one another, so that a large number of active sites is present, with the uniformity of the pore openings allowing entry of certain molecular structures relieved. It was found that K.: crystalline aluminum silicate zeolites with effective pore diameters of et -.-. a 6 to 15 »preferably 8 to 15 Angstrorn units in combination with the platinum group metal and especially after one Base exchange to reduce the amount of AlKalioxio (z.ii. iia ^ O) of the zeolite to less than about 1% Gow.-; very are effective hydrocracking catalysts.

Further hydrogenation catalysts contain a hetali from the Group VIII of the periodic table, e.g. nickel, cobalt, Luisen

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or a metal from the platinum group, e.g. palladium, platinum, Iridium or ruthenium, on a suitable support. Preferably "there is generally a Cxid oo.er ob If id one Group \ TIII metal (especially iron, cobalt or Winding) mixed with an oxide or sulfide of a metal from group VIB (preferably molybdenum or tungsten). Suitable ■ j} carriers are e.g. acidic carriers such as silicon dioxide - aluminum oxide - oleiciumdioxide-megagnesium oxide, so; the other well-known carriers for gracKungskatalysatoren; the sour ϊοηβ; fluorinated Alumina; and mixtures "of inorganic oxides, e.g. Aluminum oxide, silicon dioxide, zirconium dioxide, and titanium dioxide, with sufficient acidic properties to ensure effective graying.

i'erner can use the various metals and metal oxides and -sulfide applied to a mixture of carrier materials will. For example, 3. a /> eolite and an aluminum oxide in different proportions are caught as carrier material with each other ν, these I carrier materials different May have metals in iPorrn deposited thereon.

Typical examples of browning catalysts are the various commercially available catalysts, for example "Davison XZ-25", "Aerocat Triple S- ^ ¹¹ ," Iialcat KSi? "," Rioudry "Z-1" etc. These catalysts are grounded of a silica-alumina zeolite 'carrier' mass in rake sizes of usually 0.14 mm to 9.2 mm, suitably from 1.87 to 5.175 mm; and contain the oxides of Rare Earth.

Some typical compositions of the catalysts are given below. "I) Avison XZ-25", a Irodukt the Davison Chemical Company, is a ürackun ^r; skatalysator with a mixed oiliciuff'aioxid-Äluminiumoxid zeolite i'räger which is approximately 'jQ to 3p wt .- ^ alumina, 18 Wt .- ^ aeolite X and

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contains about 2 % by weight of ger and 1% by weight of lanthanum. ".aerocat rriple Ö-4", a 1rodnKt of the American Oyyna ^ id Company, is a bixiciu. ;; uioxid- ^ lUii; iniui.io: tid-.jeolitn-Crcc ^ un ;;: siiataljSator, aev about> _ : ew.- .. /-lir.iniuv-oxid, 5 wt .---; ^ eolite Y, 0.5 wt. Ger un-.ie, 1 wt .- /, contains innthan. "i: - = lcat LSF", a j: TO (l.iu; t the i.aico ühcuicsl Go. is a Siiiciuudioxid-Aluffiinium-

olitn-Grcickunr-skatalysetor, which is about J1 - 35 wt .-, · iiij umoxid, 11 Gev; .-, .- j /.■eolite X, about 1 "ew.- ·· cerium and 0.3 wt .-, x len ^ IiMP contains.

This process is particularly [.suitable for ii ^ -v i'ierun ■ sn'oi-driving, in particular, for example, for the petroleum fractions in the form of low viscosity, ice oils and with solution. .-. '" duiool - e leads, with a scinvcfelfest ι yörierun ^ s catalyst in the presence of ' -.metal from the l-lfitinpruppe ruf contains aluminum oxide, uit '.; assersboff is treated.

The Hydrogen Benandlunr; In the first oouf, a ratio of the hourly units of weight used is generally given by a ratio of the hourly units of weight used: anj; .- snav - rial per weight unit kotalysator (gives way to hourly space velocity, V / HSV) from about 0.1 to C, j and a V / water amount of about 0.1? 6 - 0.890 vP / 1 ( 10OU - ^ oOOü scf / b.) Carried out. Venn ax first hydrogen treatment; to give a technical oil, which are preferred iteaktionsbedinguna-en ierperaturen of 316 - 3 1 ⁰ C, about 10> - 211 atm pressure, a ΥΛΥ6Υ ü of about 2 to 0.5 and a '.iasserstoffmenge of about C, 1 ^r / b - 0, ^ 34 - ra ^ / 1 (1000 - 3000 scf / b.). i) io bevorsup-ten,> ediiK: ounces zur ^ rzeir'UiK of an Ulf; of iiahi'unrsiättelgüte, on the other hand, iOi ^ oerfturen of

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about 34-3 - 505 ⁰ C, pressures of about 155 - 35 ^ atü, a V / IISV of about 0.15-0.55 and an amount of hydrogen of about 0.267 G, c90 v? / \ (15OÜ - 5000 scf / b.).

The hydrogenated ul from the first stage is then subjected to less severe reaction conditions, e.g. temperatures of about 232 ⁰ G (or about 54-3) to 3c> 5 C, pressures of about 155 - 352 atmospheres, a UIISV of about 0, 15 (or even about 0.25) to 0.75 and an amount of hydrogen of about 0.089-0, d90 m / 1 (500-5000 scf / b.) · In order to create the less intense reaction conditions, the temperature in Average in the second hydrogenation stage - at least about 30 ° C., preferably about 4-0 G lower than in the first hydrogenation stage. The preferred range of .Ueaktionsbeding-uiig; s lies in the production of technical Ul at temperatures of 274- - 34-3 U, pressures of about 70 - 211 atmospheres, a ViLSV of about 0.25 - O, 5 ₅ una ' Hydrogen quantities of about 0.09 0.534-m ^J / l (.7OO - 500C scf / b.). If a food grade oil is to be produced, the preferred environmental conditions are temperatures of about 232 (or about 260) to 330 ⁰ O, pressures of about 141 - 352 atmospheres, a WhSV of about 0.15 (or even about 0.25) to c, p5 and amounts of hydrogen of about 0.267 m ^ / 1 (15ΟΟ - 5OCO scf / b.).

As a catalyst for the first hydrogen treatment, anyone can Sulfur-resistant Kichtedelmetall-IIydrierunf'okcitylync ^ tor used some of which are usually used in the case of Heavy oils are used. Examples of suitable catalytic Components are tin, vanadium, metals from group 7IB of the l-eriodens ^ stems of the elements, i.e. chromium, holybdini or V.'olfrem, and lethal from the iron group, i.e. iron, Cobalt, i <ickel. These metals are often found in catalytically active caiaen l. are present in quantities, e.g. about 2 to 30 wt. / b, whereby they as ^ xides, sulfides or in another j ^ orm. Wicked Λ ^ οη m-teriulia can be used, e.g. form or compounds from the oxides or sulfides of

109841/1852 ^{ÖAD 0RföiNAL}

Group VIB metals very satisfactory catalysts. Examples of such mixtures or compounds are nickel molybdate, tungstate or chromate (or thiomolybdate thiotungstate or thiochromate) or mixtures of nickel or cobalt oxide with molybdenum, tungsten or chromium oxide. It is known that these catalysis components are generally used on a support made of a solid, refractory oxide, for example on predominantly calcined or activated aluminum oxide. The commonly used catalysts containing a metal from the iron group and 5 ois 25 'io of a metal from Group VIB (calculated as oxide) is about 1 to 10%. Cobalt molybdate or nickel molybdate on aluminum oxide are particularly advantageous catalysts.

As indicated above, the catalyst for the second hydrogenation stage contains a platinum group metal. In contrast to the hydrogenation catalysts used in the first hydrogenation stage, this catalyst is normally not considered to be sulfur-resistant. The catalyst contains catalytically effective amounts of the metal from platinum group VIII, for example platinum, palladium, rhodium or iridium, which are usually in the range from about 0.01 to 2% by weight, preferably about 0.1 to 1% by weight 6, are present. The platinum group metal can be in metallic form or as a sulfide, oxide, or some other compound. The metal can possibly form compounds with other components of the catalyst, but if the metal from the platinum group is in metallic form during its actual use, it should be so finely divided that it cannot be detected by X-ray diffraction, ie it should be in Form of smallest crystals with a size of less than about 50 S are present. Platinum is preferred among the bales of platinum; if desired, the catalysts of the first and second hydrogenation can be purified with hydrogen or prereduced by heating them in the presence of hydrogen before use

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usually on l'emperaturen of about 14-9 - 316 ⁰ C for .Cleaning or 316 - 4-27 G to previous reduction.

Although various of the solid, refractory 'embossers as tracers for retail from the platinum group can be used is the preferred carrier predominantly of the annealed or activated type alumina. The alumina matrix is usually the main ingredient of the catalyst and makes at least about 75 wt. preferably at least about δ5-99, δ% by weight, based on the Catalyst, off. The alumina matrix of the catalyst can be an activated or gamma aluminum oxide, aluminum oxide monohydrate, Be alumina trihydrate or a mixture thereof. An advantageous catalyst support is a mixture that a major proportion of about 65-95% by weight of one or more the aluminum oxide trihydrates, a bayerite I, udstrandite or Gibbonite, and about 5 to 35 wt. Aluminum oxide monohydrate (Boehmite), amorphous, hydrous aluminum oxide or a Contains mixture thereof. The aluminum oxide carrier can contain small amounts of other solid oxides, e.g. silicon dioxide, magnesium oxide, natural or activated clays (e.g. kaolinite, hontmorillonite, lalloysite, etc.), titanium dioxide, zirconium dioxide, usxv. or mixtures thereof.

The invention is further illustrated by the following examples, however, these are not intended to limit the invention.

example 1

A vertical steel cylinder with a diameter of 10.16 cm and a length of 12.2 m, the one with a cradle for the catalyst was fitted with a pre-screened, extruded nickel-molybdenum catalyst with a diameter of 1.5ö7 mm. The catalyst was on Removal of the debris has been pre-screened by placing it on a

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liO-Btaiidc'osieb von ? .O i: esn 'was sieved.

her catalyst · v.-cie iicer den ^ uerschnir.ijs area des ^ ylincier: -5 i :: it ". --iner Geoc'm -. 'indi _K: eit of? 6.2 rm per kinute about oim- Mi j-xb ^ t-'iid. Vo ^. Etv>:? 1_, 2 to 11, \ u dropped freely, whereby oj.c L ^ υ ± ι ^ stort-eilp.hen nich v / rUirend the formation des ί \ · tal ^ PRtoL'be-ct ^ n - ^ loichmu ^ ifT distributed, all in all ^ 'ItX ¹ ■ "des Lnt;? iysa-Gors were filled into the / jylinder, r.ach the Liutcabo uuo 1. · λ üalysators v; urde the replaced abrasion in Ggv: - j L: estii..ii> _T inaem the! »analyzer called a ^ l Kesn-oieb geoiebü. Dor abrasion be ^r : ruf C, pb wt.

'under ver \ .endun; -left, whereby a "sock" -2eschicKun - s procedure siv.iuiiert \; urae. Ü-rr.Arrisb rerrug in these ^ aIIe G, ^: Gev. ⁷ .—: - ·,

biiter Ver · ..endune of a cylinder with a diameter of h:;:, v c: .i and a length of 6.1 π was the catalyst of iseis ^ iel 1 using a conical distributor for Lraeuguiu of a catalyst! ".. 'it is evenly distributed on (joreben. Laughing the jilaung of the catalyst bed was the Alignment: of the kaualysato_teilcnen by ^ eobacntunc: determined; she was iih v: a sent lic hen horizontal.

l; ii the i'estif: -kei "fc of the Kaoalysaüorbetües produced in _; eis iel 2 to ermirtelii, an o,: / v '..na-steel rod was reholt and dtnn over ai-3 iVotaiyGCttorocerflache. The οΌογ, dranr ^, ^ - ^; > ei. Deep a. Iiin zw-ices K -.- ^ slysatc'rbett v; urde iv "- 7en \: hre- as in ^ eisydel 1 evzeu-rc. ~ ucv

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ο.35 rarn-otahl rod was placed vertically over the catalyst surface held and released. It penetrated 30.5 cm.

example

In this example, a steel tower with a diameter of 4 cm and a length of 6.1 tons was used, which was equipped with I-iisch- and feed devices for liquids and nitrogen gas at the top of the tower and the one at the bottom des Turues had traps divided into sections, polygons consisted of nine sections to determine the distribution of the liquid flow and the distribution of the residence time for differently formed catalyst beds using a tritiated i-thylcyclohexane tracer The feeding device at the top of the tower used in the following examples was either a flat disk with a diameter of 4-0.6 cm ... or a concentric pan, from which the liquid in two concentric circles into the Bed could flow. The collecting device θιά bottom of the tower consisted of nine parts, which consisted of nine sections, which were separated from each other by 76.2 mm high partition walls. At the bottom of each catchment section there was a 30.1 mm high layer of 6.35 mm thick aluminum spheres. The sectioned collecting device also had outlet openings at the bottom of each section for the recovery of the liquid, and the side walls of the collecting device reached so far into the tower that the filled catalyst extended approximately 38.1 mm into each section. The nine sections of the catcher consisted of a central section that was located in the center of the catcher and had a radius of 14.9 cm. The left and right sides of the catcher were formed next to the gown section by a separator which separated the left from the right sections. The sections "ii ^ chta 3", "Right 4" (■ {*, K4-) and "Left 3", "Left ^/ f -""'(L3, L4-) were created by dividing the area by

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-, 9 cm to 33,000 cm in diameter, with sections L 3 and RJ taking up about 12.5 P of the area, and sections R4 and IA taking up about 37.5% of the area. The remaining sections, "Links 1", "Links 2" (LI, L2). and "iiecnts 1", "smells 2" (ii1, R2), were obtained aurcn. uniform area distribution of the remaining area of the collection direction, which ranged from 33 »0 cm to 4-3.2 cm, ie the outer hadius of the collection device. (The designations L1-4- and ..- ii-4- are in the below dragonfly II used). In order to determine the residence time, the inlet opening for the liquid was set up so that the tracer could be injected into the liquid, and there was also a monitoring device at the bottom of the tower in order to determine the length of the tracer following the bottom of the tower Achieved different time periods, To determine the distribution of the liquid and the residence time, a heating oil with a density of 4-2 ⁰ API and a viscosity of 1.85 Gp at 26.7 ° 0 and an extruded nickel-holybdenum catalyst were used as the catalyst

55

1.5ö7 ™ diameter and a pore volume of 0.55 used.

The following table shows the results obtained for the liquid distribution, the residence time and the bulk density were obtained, the catalyst according to the not in the In the middle of the tower carried out the "sock" -i-iethode (S), by simple Pouring (pour-down method) (P) and according to the invention (E) had been poured.

For the "sock" method, the catalyst was poured from a 76 liter funnel fitted with a flexible four-inch diameter tube which was cut into the tower with the lower end of the hose in contact with it the catalyst surface was wrinkled. The Kataiysabor was on the right side of the tower; lam ^;::; on our; thorn under -on unde of the hose flow, think, position yourself above the

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Divider between the sections _i1 and -ä'j. found.

with aet.i simple ^ ingieLen (1-) a Tl5 liter er -, / ric over, in the lower end of which there was a closure valve of '/''- was filled with your catalyst, where: j The locking valve was located above the middle of the tower; the valve was opened and the catalyst was dropped in one continuous stream onto the surface of the catalyst gate.

5 ¹ The same 76 liter funnel was used for the method according to the invention as in the "sock"method; However, it was provided with a notched plastic funnel which was suspended from a rod through the middle of the funnel. The funnel served as a valve for, closing and / or regulating the flow rate of the catalyst from the funnel and for the uniform distribution of the catalyst flow over the entire diameter of the tower. The K & öalysator was filled with a vertical filling speed of 2.5 cm / min.

In the following tables, the filling method for the catalyst, the feed device (A) when using; of the disc, (B) when using the centered pan, the amount of catalyst, the liquid and gas velocities and the percentage of the total flow indicated in the individual sections. The values for the 1 ' ¹ IuB in the individual sections have been corrected to show all Irozontangsben in the uneven i ^{; 1} lachenabscanitten on the same basis, the perfect distribution for each section should be 11.1 ^l , i . Lie jjCiiiittaichten ζ us air men η-it the number of ideal heating tanks (J) are entered, which are necessary in series in order to approximately reflect the residence time spectrum of the system.

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109841/1852

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109841/1852

The results obtained in Examples 1 to 4 show the results excellent effectiveness of the method according to the invention. In particular Example 1 shows that, according to the invention, a reactor is charged with a catalyst and thereby the formation of Can keep catalyst wear to a minimum. The strength of the catalyst bed (Example 3) is due to the slight Penetration of the steel powder into the catalyst bed clearly shown. In this way, in the case of catalyst beds produced according to the invention, the problems with regard to collapse can be overcome of the catalyst, which can damage the internal parts of the reactor and in some 3? all to complete Inability to monitor the temperature of the reactions can result. Of particular importance is Example 4-, in which the bulk density of the catalyst bed was increased in the procedure according to the invention. The bulk density is in the charging process known from the prior art, i.e. with the "sock" method and with simple pouring, only 0.61, with the charging according to the invention, however, 0.81. This remarkable increase in bulk density leads to higher efficiency and utilization of the catalyst at various Procedure. Thus, a higher throughput of reactants can be achieved, while that for one such throughput required reactor volume to a minimum can be held. In addition, the values of the liquid distribution and the residence time distribution show that with the invention In the process, a better liquid distribution was obtained is, increasing the effectiveness of the catalyst by the more uniform Distribution of the reactants over the available catalyst surface is improved. aside from that show the results of the experiments to determine the residence time distribution that a more effective catalyst bed is obtained when the catalyst is filled in according to the process of the invention.

Claims

BATH ORIGINAL

109841/1852

Claims (1)

- 21 claims 1. Method of filling a solid catalyst into a ! Fixed bed reactor, with a catalyst surface with increased Bulk density is formed while the catalyst volume with the formation of a catalyst bed in the iieaktor is filled, characterized in that the reactor rait solid catalyst particles, which have a practically cylindrical geometry, at a vertical oil velocity of up to 4-5.2 cm per foinute and at an average free fall distance of the catalyst particles through a gaseous medium to the catalyst surface of at least about 30.5 cm in downward motion is charged, with the longitudinal axis of the quay; alysatorteilchen is oriented essentially horizontally in the catalyst bed. 2- The method according to claim 1, characterized in that the Filling speed 2.5 to about 15.24 cm per hour, preferably is about 5 »0 to 10.16 cm per 1 minute. 3. The method according to claim 1 or 2, characterized in that that the free l'all distance about 1.52 to 30.1 m, preferably is about 3.0 to about 21.3 η. 4-, Verfahrsn according to claim 1, 2 or 3 »characterized in that that the catalyst particles have a diameter of about 0.794 to about 6.35 mm, preferably about 1.5 & 7 to about 3.175 mm to have. 5. The method according to claim Λ, characterized in that the Ratio of the length of the catalyst particles r; egeimoer their The diameter is about 1.5 to 6, preferably about 2 to 5 . BATH 109841/1852 b. Catalyst bed with increased,. of a iieactor, df-by reKennaeichnet, ο <;.] ".. the rusting Eni; & - lysatorteilcaen a practically syliridriscne '' ioosnobrie r.nfv.'eisen, and dal: ^r üe ii'.38i7se'r, o: ci = * 'iinäer in oesi Krnai'/:;?. gate bed in the v.'ese'r-tiichen hcri ',: ontsl PUR ^ are erected. 7. KaualysatorlDett according to claim 6, änaurch 'egg: enri2-, EIC line t, the diameter of the particles DAT ir, gereich // 94- rara of ebv-- G to 6.35, _vorzu. Sv / else about 1 , 5ό? to 5, .I ¹ / ^ ^rr -'- · li &L't, urd öaL dos "ratio of the L ^ n ^r ~ .e of the K-jcalysatorteilcaen to their diameter etvja 1, p to 6,. -preferred · -; ei se is approximately > until ^L j . 109841 MR52